Theoretical-exploration-of-seleno

Theoretical exploration of seleno and tellurophenols as
promising alternatives to sulfur ligands for anchoring to gold
(111) materials
Por:Miranda-Rojas, S (Miranda-Rojas, Sebastian)[ 1 ] ; Salazar-Molina, R (Salazar-Molina,
Richard)[ 2 ] ;Kastner, J (Kaestner, Johannes)[ 3 ] ; Arratia-Perez, R (Arratia-Perez,
Ramiro)[ 4 ] ; Mendizabal, F(Mendizabal, Fernando)[ 2 ]
RSC ADVANCES
Volumen: 6
Número: 6
Páginas: 4458-4468
DOI: 10.1039/c5ra21964g
Fecha de publicación: 2016
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Resumen
It is widely known that sulfur ligands, such as alkanethiols or phenothiols and their derivatives, are
useful anchor systems for gold materials due to the high affinity of sulfur to gold surfaces. In this
study we use DFT calculations and a 42-atom gold cluster model to study the interaction between
selenophenol and tellurophenol-derivatives with the Au(111) surface to gain information towards
potential new gold-based materials. We modulated the interaction strength by controlling the charge
transfer process of a particular interaction by chemically modifying the ligands. To obtain a
complete analysis, we studied the ligands in their protonated, anionic and radical states aiming to
cover the three possibilities in which these may interact with the gold cluster. In order to get a
deeper insight into the nature of the interaction we used several analysis techniques such as
energy decomposition analysis (EDA), non-covalent interactions (NCI) and natural population
analysis (NPA). Our results reveal that tellurium in the anionic state provides complexes of better
thermodynamic stability by similar to 12.0 kcal mol, when compared with the strongest sulfur-gold
complex, also in the anionic state. Furthermore, this indicates that the anionic ligand is probably the
dominant state for both selenium and tellurium as observed previously for sulfur. The extent to
which the interaction strength could be controlled directly depends on the state of the anchor atom.
In our case the anionic state is the most suitable for tuning the interaction. Finally, our main findings
suggest that exchanging sulfur with selenium or tellurium involves an important increase of the
interaction strength, thus, making these selenophenol and tellurophenol derivatives attractive for the
development of new functional materials.
Palabras clave
KeyWords Plus:SELF-ASSEMBLED MONOLAYERS; CHELATING DIARYLOXO
LIGANDS; TITANIUM COMPLEXES; FORCE MICROSCOPY; CHARGE-TRANSFER; CHAINLENGTH; BASIS-SETS;CHEMISTRY; SURFACES; PSEUDOPOTENTIALS
Información del autor
Dirección para petición de copias: Miranda-Rojas, S (autor para petición de copias)
Univ Andres Bello, Fac Ciencias Exactas, Dept Ciencias Quim, CPC, Ave Republ 275, Santiago,
Chile.
Dirección para petición de copias: Salazar-Molina, R (autor para petición de copias)
Univ Chile, Fac Ciencias, Dept Quim, POB 653, Santiago 3425, Chile.
Direcciones:
[ 1 ] Univ Andres Bello, Fac Ciencias Exactas, Dept Ciencias Quim, CPC, Ave Republ 275,
Santiago, Chile
[ 2 ] Univ Chile, Fac Ciencias, Dept Quim, POB 653, Santiago 3425, Chile
[ 3 ] Univ Stuttgart, Inst Theoret Chem, Pfaffenwaldring 55, D-70569 Stuttgart, Germany
[ 4 ] Univ Andres Bello, Relativist Mol Phys ReMoPh Grp, Ctr Nanociencias Aplicadas, Fisicoquim
Mol,CENAP, Republ 275, Santiago, Chile
Direcciones de correo electrónico:sebastian.miranda@unab.cl
Financiación
Entidad financiadora
Número de concesión
FONDECYT
3130383
1140503
1150629
Grant ICM
120082
CONICYT
21130874
German Research Foundation (DFG)
EXC 310/2
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Editorial
ROYAL SOC CHEMISTRY, THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD,
CAMBRIDGE CB4 0WF, CAMBS, ENGLAND
Categorías / Clasificación
Áreas de investigación:Chemistry
Categorías de Web of Science:Chemistry, Multidisciplinary
Información del documento
Tipo de documento:Article
Idioma:English
Número de acceso: WOS:000369510500023
ISSN: 2046-2069
Información de la revista
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Impact Factor: Journal Citation Reports®
Otra información
Número IDS: DC8ZT
Referencias citadas en la Colección principal de Web of Science: 52
Veces citado en la Colección principal de Web of Science: 0